Development strategies and improved photocatalytic CO_(2) reduction performance of metal halide perovskite nanocrystals

In recent years,photocatalytic CO_(2)reduction reaction(CRR) has attracted much scientific attention to overcome energy and environmental issues by converting CO_(2)into high-value-added chemicals utilizing solar energy.Metal halide perovskite(MHP) nanocrystals(NCs) are recognized as an ideal choice for CRR owing to their outstanding optoelectronic properties.Although great efforts have been devoted to designing more effective photocatalysts to optimize CRR performance,severe charge recombination,instability,and unsatisfactory activity have become major bottlenecks in developing perovskite-based photocatalysts.In this review,we mainly focus on the recent research progress in the areas of relevance.First,a brief insight into reaction mechanisms for CRR and structural features of MHPs are introduced.Second,efficient modification approaches for the improvement of the photocatalytic activity and stability of the perovskite-based catalysts are comprehensively reviewed.Third,the state-of-the-art achievements of perovskite-based photocatalysts for CRR are systematically summarized and discussed,which are focused on the modification approaches,structure design,and the mechanism of the CO_(2)reduction process.Lastly,the current challenges and future research perspectives in the design and application of perovskite materials are highlighted from our point of view to provide helpful insights for seeking breakthroughs in the field of CRR.This review may provide a guide for scientists interested in applying perovskite-based catalysts for solar-to-chemical energy conversion.

Structural design for electrocatalytic water splitting to realize industrial-scale deployment: Strategies, advances, and perspectives

The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the global average temperature rise in the range of 1.5–2.0 ℃ above the pre-industrial level by the end of this century. Tremendous efforts have been devoted to the optimization of the electrocatalytic performance of the catalysts under industrial-relevant current densities via rational structure design,which induces a preferential electron distribution that favors the adsorption/desorption behavior of the key intermediates, thus accelerating the reaction kinetics. In this review, a brief introduction of the current energy status will be first presented to necessitate the importance of green hydrogen.Followed by the basic concepts and fundamental understanding of the reaction mechanisms, we present efficient strategies for the enhancement of the electrocatalytic performance of the catalysts to meet the rigorous requirement under industrial conditions and the in-depth understanding behind the reinforcement will be briefly discussed next. Then the recent advances regarding the rational design of electrocatalysts operating at an industrial scale will be summarized. Finally, the challenges and perspectives in this thriving field will be proposed from our point of view.

Highly stable lead-free Cs3Bi2I9 perovskite nanoplates for photodetection applications

Lead halide perovskites have received tremendous attentions recently for their excellent properties such as high light absorption coefficient and long charge carrier diffusion length. However, the stability issues and the existence of toxic lead cations have largely limited their applications in optoelectronic area. Herein, we report the synthesis and investigation of highly stable and lead-free Cs3Bi2I9 perovskite nanoplates for visible light photodetection applications. The Cs3Bi2I9 nanoplates were synthesized through a facile solution-processed method, which is also applicable to various substrates. The achieved nanoplates present very good crystal quality and exhibit excellent long-term stability even exposed in moist air for several months. Photodetectors were constructed based on these high-quality perovskite nanoplates for the first time, and display a maximum photoresponsivity of 33.1 mA/W under the illumination of 450 nm laser, which is six times higher than the solution-synthesized CH3NH3PbI3 nanowire photodetectors. The specific detectivity of these devices can reach up to 10^10 Jones. Additionally, the devices exhibit fast rise and decay time of 10.2 and 37.2 ms, respectively, and highly stable photoswitching behavior with their photoresponse well retaining under alternating light and darkness. This work opens up a new opportunity for stable and low-toxic perovskite-based optoelectronic applications.

非周期性原子排列实现电化学氮还原和析氧反应性能的增强

制备低成本的高效电催化剂是缓解目前面临的环境能源危机的重要方式.通过无定型化和构建异质结构可以有效地改变催化剂的电子结构,从而实现电催化性能的稳步提升.但是对于两者之间协同作用的研究则相对较少.在本文中,我们构建了富含异质结构的无定型FeMo基(a-FeMo)电催化剂,并系统评估了该催化剂的氮气还原和析氧反应性能.得益于无定型结构引起的活性位点数目的增多和异质结构引发的电子的重新分布,a-FeMo催化剂表现出优异的电化学催化性能.在-0.1 V vs.RHE的电势下,a-FeMo催化剂表现出29.15%的法拉第效率和71.78μg_(NH_(3)) mg_(cat.)^(-1) h^(-1)的氨气产率.这为合理设计具有低成本优势、高活性和长时间稳定性的优异催化剂提供了有益的参考.